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Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal-Organic Framework.
Ikuno, Takaaki; Zheng, Jian; Vjunov, Aleksei; Sanchez-Sanchez, Maricruz; Ortuño, Manuel A; Pahls, Dale R; Fulton, John L; Camaioni, Donald M; Li, Zhanyong; Ray, Debmalya; Mehdi, B Layla; Browning, Nigel D; Farha, Omar K; Hupp, Joseph T; Cramer, Christopher J; Gagliardi, Laura; Lercher, Johannes A.
Afiliación
  • Ikuno T; Department of Chemistry and Catalysis Research Institute, Technische Universität München , 85748 Garching, Germany.
  • Zheng J; Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
  • Vjunov A; Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
  • Sanchez-Sanchez M; Department of Chemistry and Catalysis Research Institute, Technische Universität München , 85748 Garching, Germany.
  • Ortuño MA; Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota , Minneapolis, Minnesota 55455, United States.
  • Pahls DR; Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota , Minneapolis, Minnesota 55455, United States.
  • Fulton JL; Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
  • Camaioni DM; Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
  • Li Z; Department of Chemistry, Northwestern University , Evanston, Illinois 60208, United States.
  • Ray D; Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota , Minneapolis, Minnesota 55455, United States.
  • Mehdi BL; Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
  • Browning ND; Institute for Integrated Catalysis, and Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
  • Farha OK; Materials Science and Engineering, University of Washington , Seattle, Washington 98195, United States.
  • Hupp JT; Department of Chemistry, Northwestern University , Evanston, Illinois 60208, United States.
  • Cramer CJ; Department of Chemistry, Faculty of Science, King Abdulaziz University , Jeddah 21589, Saudi Arabia.
  • Gagliardi L; Department of Chemistry, Northwestern University , Evanston, Illinois 60208, United States.
  • Lercher JA; Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota , Minneapolis, Minnesota 55455, United States.
J Am Chem Soc ; 139(30): 10294-10301, 2017 08 02.
Article en En | MEDLINE | ID: mdl-28613861
Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal-organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu+ and ∼85% Cu2+. The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu2+ to Cu+. The products, methanol, dimethyl ether, and CO2, were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45-60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2017 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Estados Unidos
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2017 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Estados Unidos